Mean Streets (1973)
The early De Niro walks the tightrope between gritty and seductive. In Mean Streets, he has a kind of shaggy, bruised matinee idol look, but he's blowing up mailboxes and ruining Harvey Keitel's plans. Is this how a heart-throb behaves? So, cute or crazy?

Mean Streets, Robert De Niro, 1973. Photo courtesy of the Everett Collection.